Abstract
Simulation of the rotational envelopes of the lowest-energy Rydberg R6s transitions of methyl iodide for one- and two-photon resonant absorption processes indicates that the spin of the Rydberg electron is uncoupled from the molecular axis. This result, which is somewhat unexpected, resolves several inconsistencies in previous interpretations of the rotational sub-band structure of these spectroscopically important transitions.
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